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通过胺功能化 Cu-BTC 对 CO 吸附实现富氢合成气升级:不同胺的影响。

Hydrogen-rich syngas upgrading via CO adsorption by amine-functionalized Cu-BTC: the effect of different amines.

机构信息

Institute of Energy and Power Engineering, Zhejiang University of Technology, Hangzhou, 310014, China.

Zhejiang Energy Group, Hangzhou, 310014, China.

出版信息

Environ Sci Pollut Res Int. 2024 May;31(24):35979-35991. doi: 10.1007/s11356-024-33646-7. Epub 2024 May 15.

Abstract

Syngas produced from supercritical water gasification typically contain a high amount of CO along with H. In order to improve the quality of syngas, amine-functionalized copper benzene-1,3,5-tricarboxylate (Cu-BTC) was synthesized as an effective adsorbent for selective removal of CO from syngas to increase the concentration of H. The amines used in this study included monoethanolamine (MEA), ethylenediamine (EDA), and polyethyleneimine (PEI). The fundamental physicochemical character of adsorbents, CO adsorption capacity, and CO/H selectivity were analyzed. The physicochemical characterization indicated that the structure of amine-functionalized Cu-BTC was partially damaged, which resulted in a decrease in specific surface area and pore volume. On the other hand, the enlarged pore size was beneficial for the mass transfer of gas in the adsorbent. Among these adsorbents, Cu-BTC/PEI exhibited the maximum CO adsorption capacity of 3.83 mmol/g and the highest CO/H selectivity of 19.74. It was found that the adsorption pressure is the most significant factor for the CO adsorption capacity. Lower temperature and higher pressure were favored for CO adsorption capacity and CO/H selectivity, so physical adsorption by Cu-BTC played a dominant role. Moreover, Cu-BTC/PEI can be well-regenerated with stable adsorption efficiency after five consecutive cycles. These findings suggested that Cu-BTC/PEI could be a promising alternative adsorbent for CO capture from syngas.

摘要

由超临界水气化产生的合成气通常含有大量的 CO 和 H。为了提高合成气的质量,合成了胺功能化的铜苯-1,3,5-三甲酸酯(Cu-BTC)作为一种有效的吸附剂,用于从合成气中选择性地去除 CO,以提高 H 的浓度。本研究中使用的胺包括单乙醇胺(MEA)、乙二胺(EDA)和聚乙烯亚胺(PEI)。分析了吸附剂的基本物理化学性质、CO 吸附容量和 CO/H 选择性。物理化学特性表明,胺功能化 Cu-BTC 的结构部分受损,导致比表面积和孔体积减小。另一方面,增大的孔径有利于气体在吸附剂中的传质。在这些吸附剂中,Cu-BTC/PEI 表现出最大的 CO 吸附容量为 3.83mmol/g 和最高的 CO/H 选择性为 19.74。研究发现,吸附压力是 CO 吸附容量的最显著因素。较低的温度和较高的压力有利于 CO 吸附容量和 CO/H 选择性,因此 Cu-BTC 通过物理吸附起主要作用。此外,Cu-BTC/PEI 在经过五个连续循环后可以很好地再生,并保持稳定的吸附效率。这些发现表明,Cu-BTC/PEI 可以作为从合成气中捕获 CO 的一种很有前途的替代吸附剂。

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